We have investigated functionalized 2D carbon allotrope, graphdiyne (GDY), as a promising hydrogen storage media. Density functional theory with a range of vdW corrections was employed to study Ni decoration of pristine and boron-doped GDY and the interaction of resulting structures with molecular hydrogen. We showed that boron-doped GDY is thermally stable at 300 K, though, its synthesis requires an endothermic reaction. Also, boron doping enhances Ni binding with the graphdiyne by increasing the charge transfer from Ni to GDY. Ni doping drastically influenced hydrogen adsorption energies: they rise from ~70 meV per H₂ molecule on pristine GDY to a maximum of 1.29 eV per H₂ becoming too high in value for room temperature reversible applications. Boron doping improves the situations: in this case, after Ni decoration desorption temperature estimation is ~300–500 K. Overall, each Ni adatom on B-doped GDY can bind only one H₂ molecule within the needed energy range, which gives low hydrogen uptake (~1.2 wt%). However, doping with boron led to the decrease in the value of hydrogen adsorption energy and good desorption temperature estimations, therefore, codoping of metal atoms and boron could be an effective strategy for other transition metals.

我们已经研究了功能化的2D碳同素异形体graphdiyne（GDY），它是一种很有前途的储氢介质。使用具有一定vdW校正范围的密度泛函理论来研究原始和掺硼GDY的Ni装饰以及所得结构与分子氢的相互作用。我们表明，掺硼的GDY在300 K时具有热稳定性，尽管其合成需要吸热反应。而且，硼掺杂通过增加从Ni到GDY的电荷转移来增强Ni与石墨二炔的结合。镍掺杂大大影响氢吸附能：它们从〜70兆电子伏每股H上升₂分子上原始GDY到最大1.29电子伏特的每股H ₂对于室温可逆应用而言，其价值变得过高。硼掺杂改善了这种情况：在这种情况下，估计的Ni装饰解吸温度约为300-500K。总体而言，B掺杂GDY上的每个Ni原子只能结合所需能量范围内的一个H ₂分子，从而产生低氢摄取（〜1.2 wt％）。然而，硼的掺杂导致氢吸附能值的降低和良好的解吸温度估算，因此，金属原子与硼的共掺杂可能是其他过渡金属的有效策略。